NMR and EPR studies of chloroiron(III) tetraphenyl-chlorin and its complexes with imidazoles and pyridines of widely differing basicities.

Inorganic Chemistry
Sheng CaiF Ann Walker

Abstract

The NMR and EPR spectra of two bisimidazole and three bispyridine complexes of tetraphenylchlorinatoiron(III), [(TPC)Fe(L)2]+ (L = Im-d4, 2-MeHIm, 4-Me2NPy, Py, and 4-CNPy), have been investigated. The full resonance assignments of the [(TPC)Fe(L)2]+ complexes of this study have been made from correlation spectroscopy (COSY) and nuclear Overhauser enhancement spectroscopy (NOESY) experiments and Amsterdam density functional (ADF) calculations. Unlike the [(OEC)Fe(L)2]+ complexes reported previously (Cai, S.; Lichtenberger, D. L.; Walker, F. A. Inorg. Chem. 2005, 44, 1890-1903), the NMR data for the [(TPC)Fe(L)2]+ complexes of this study indicate that the ground state is S = 1/2 for each bisligand complex, whereas a higher spin state was present at NMR temperatures for the Py and 4-CNPy complexes of (OEC)Fe(III). The pyrrole-8,17 and pyrroline-H of all [TPCFe(L)2]+ show large magnitude chemical shifts (hence indicating large spin density on the adjacent carbons that are part of the pi system), while pyrrole-12,13-CH2 and -7,18-CH2 protons show much smaller chemical shifts, as predicted by the spin densities obtained from ADF calculations. The magnitude of the chemical shifts decreases with decreasing donor ability of the substit...Continue Reading

References

Mar 28, 1977·Biochimica Et Biophysica Acta·E A PermyakovI Yamazaki
Aug 22, 1997·Biochimica Et Biophysica Acta·S Jünemann
Nov 15, 2000·Biochemistry·A JasaitisM I Verkhovsky
Nov 5, 2003·Nature Structural Biology·M Elizabeth StroupeElizabeth D Getzoff
Dec 18, 2003·Journal of the American Chemical Society·Liliya A YatsunykF Ann Walker
Sep 15, 2004·The Journal of Biological Chemistry·Tobias W B OstStephen K Chapman
Apr 12, 2005·Inorganic Chemistry·Liliya A YatsunykF Ann Walker

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Citations

Jun 25, 2010·Journal of the American Chemical Society·Matthew D LiptakKara L Bren
Jul 27, 2011·Proceedings of the National Academy of Sciences of the United States of America·Shin-ichi J TakayamaA Grant Mauk
Aug 15, 2012·The Journal of Biological Chemistry·Georgia UkpabiMichael E P Murphy

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